CN106903158B - Soil oxidation-solidification stabilization remediation agent and using method thereof - Google Patents
Soil oxidation-solidification stabilization remediation agent and using method thereof Download PDFInfo
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- CN106903158B CN106903158B CN201710124748.6A CN201710124748A CN106903158B CN 106903158 B CN106903158 B CN 106903158B CN 201710124748 A CN201710124748 A CN 201710124748A CN 106903158 B CN106903158 B CN 106903158B
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- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
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Abstract
The invention discloses a soil oxidation-solidification stabilization restoring agent and a using method thereof. According to the invention, through the molecular oxygen activation process in the zero-valent iron and disilicate system, the organic matters in the polluted soil are oxidized and removed, the interference of the organic matters on the soil solidification and stabilization process is reduced, and meanwhile, the mobility of the heavy metal polluted soil is greatly reduced through oxidation on the reductive substances such as arsenite radicals, selenite radicals and sulfide ions which may exist in the heavy metal polluted soil. Then, calcium oxide/calcium hydroxide is added, and the heavy metal ions (copper, lead, cadmium, mercury and the like) are stabilized and immobilized through iron minerals formed by residual zero-valent iron, calcium silicate compounds and the like. The remediation agent can be used for carrying out oxidation-solidification stabilization on heavy metal contaminated soil or organic matter and heavy metal combined contaminated soil with different pollution degrees, and products after solidification stabilization can be backfilled or used for other purposes.
Description
Technical Field
The invention belongs to the technical field of environment, and particularly relates to a soil oxidation-solidification stabilization remediation agent and a use method thereof.
Background
With the acceleration of the industrialization process in China, the rapid development of the industry improves the material culture living standard of human beings on one hand and causes serious environmental pollution on the other hand. Heavy metal pollution of soil is a great problem of environmental pollution. Soil is an important component of the ecological environment, is one of the most valuable resources on which human beings live, and is regenerated very slowly. Due to the discharge of domestic sewage, pollution irrigation, atmospheric sedimentation, mining and smelting, the use of a large amount of pesticides and fertilizers and the like, the soil pollution, particularly the heavy metal pollution, is getting more and more serious. Heavy metals entering the soil are nondegradable and are accumulated in the soil continuously, so that the soil heavy metals are difficult to treat due to pollution, and an economic and effective treatment method is not found up to now. Heavy metals deposited in the soil can enter the plant body through the soil-plant ecosystem to be accumulated, so that the growth and development of crops are retarded, the yield is reduced, the heavy metals can be absorbed by the plants and enriched at edible parts, and serious harm is caused to human health.
For the treatment of pollution caused by heavy soil, extensive research work is carried out in all countries in the world. Because the heavy soil belongs to pollution and has the characteristics of potential, irreversibility, long-term property, serious consequence and the like, the pollution treatment is based on the basic policy of 'preventing and treating more than treating'. At present, the heavy metal pollution treatment has two main ways: (1) changing the existing form of heavy metal in soil to fix the heavy metal, and reducing the mobility and bioavailability of the heavy metal in the environment; (2) heavy metals are removed from the soil. The methods adopted at home and abroad generally comprise a physical chemical method and a biological method, and the treatment methods have various advantages and disadvantages. Among these, the curing and stabilizing technique is a more common repairing method.
The soil solidification and stabilization technology refers to a group of restoration technologies for preventing or reducing the process of releasing harmful chemical substances from the polluted soil, and is generally used for harmless treatment of the soil polluted by heavy metals and radioactive substances. The curing stabilization technique encompasses two concepts. Wherein, the solidification means that the pollutants are coated to be in a granular or massive state, so that the pollutants are in a relatively stable state; stabilization refers to the conversion of a contaminant into a form that is not readily soluble, has reduced migratory capacity or toxicity, i.e., by reducing the biological effectiveness of the contaminant, rendering it harmless or reducing the risk of its harmfulness to the ecosystem. The curing and stabilizing effect on metal pollution is obvious, destructive technology does not exist, and the method can be adopted for As, Pb, Cr, Hg, Cd, Cu and Zn. The solidification and stabilization technology can be used for digging out the polluted soil, mixing the polluted soil on the ground, putting the mixture into a mold with a proper shape or placing the mixture into an open space for stabilization treatment, and can also be used for in-situ stabilization treatment on the polluted soil.
However, the existing soil remediation technologies for solidification and stabilization generally do not have an oxidation effect, are difficult to treat organic-heavy metal composite contaminated soil, and cannot achieve a stabilization effect on metal sulfides with redox activity, so that innovation is needed.
Disclosure of Invention
In order to overcome the defects in the prior art, the invention provides an oxidation-solidification stabilization restoration agent consisting of zero-valent iron, silicate and calcium oxide, which realizes the oxidation effect through a zero-valent iron and silicate system, removes organic matters in polluted soil and reduces the interference of the organic matters on the solidification stabilization process; and then adding calcium oxide, and realizing solidification and stabilization of heavy metals in the soil through the generated iron minerals and calcium silicate compounds.
The technical scheme provided by the invention is as follows:
A soil oxidation-solidification stabilization repairing agent comprises the following components: zero-valent iron powder, soluble silicates and calcium salts; the three components are packaged independently.
The zero-valent iron powder is nano zero-valent iron or micron zero-valent iron.
The soluble silicate is metasilicate or disilicate.
The calcium salt is calcium oxide, calcium hydroxide, calcium chloride or calcium sulfate.
A method for restoring soil by using the soil oxidation-solidification stabilization restoring agent comprises the following steps: firstly, preparing soluble silicate into silicate solution, then adding the silicate solution and zero-valent iron powder into soil to be repaired, and carrying out aeration stirring for more than 0.5 h; then adding a calcium source gradually, and continuing stirring; after stirring, digesting and forming the slurry, naturally cooling and crushing the slurry to obtain the cement.
The addition amount of the zero-valent iron powder in each kilogram of soil to be repaired is 0.5-10 g.
The addition amount of silicate in each kilogram of soil to be repaired is 0.1-5 g calculated by silicon atom.
The soil to be repaired is heavy metal contaminated soil or organic matter-heavy metal combined contaminated soil.
The principle of the invention is as follows:
Firstly, adding silicate solution and ferrous iron into soil to be repaired, and carrying out stirring reaction to realize oxidation of organic matters, reduce the content of organic pollutants in the soil and simultaneously reduce the interference of the organic matters on the solidification and stabilization process; then calcium oxide is added, and the stabilization and immobilization of heavy metal ions are realized through iron minerals formed by residual zero-valent iron, calcium silicate compounds and the like. For heavy metal polluted soil with reducing substances such as arsenite, selenite, sulfide ions and the like, the immobilization efficiency can be further improved by the oxidation process, for example, the mobility of the arsenite is greatly reduced after the arsenite is oxidized; after the sulfide ions are oxidized, the metal ions are released and combined with the silicate, so that the stability is increased, and the risk of secondary release of the sulfide ions oxidized into sulfate radicals can be avoided.
The specific oxidation mechanism is that zero-valent iron is oxidized into ferrous ions, the ferrous ions and silicate form a silicate-ferrous complex, the ferrous ions in a coordination state have a lower oxidation-reduction potential and can react with oxygen molecules more easily, oxygen is firstly reduced into superoxide anions, then the superoxide anions are further reduced into hydrogen peroxide, the hydrogen peroxide and the ferrous ions react through Fenton to generate a large amount of hydroxyl radicals, and the hydroxyl radicals are used as radicals with extremely strong oxidation performance and can almost remove organic pollutants in soil through nonselective oxidation. After the process is finished, calcium oxide is added into the mixture, the addition of the calcium oxide can destroy the matching state of ferrous/ferric ions and silicate radicals to generate precipitates of calcium silicate compounds, and simultaneously the ferrous/ferric ions and the residual zero-valent iron generate various iron minerals, so that the stabilization and immobilization of heavy metal ions are realized. Meanwhile, due to the oxidation effect in the process, some heavy metals in a low valence state, such as trivalent arsenic, can be oxidized into hexavalent arsenic, and the hexavalent arsenic has lower toxicity and weaker mobility than the trivalent arsenic. Some of the heavy metals, which are fixed in the form of sulfides, will be converted to exist in a stable form as silica, iron compounds.
The invention has the following advantages and beneficial effects:
(1) The soil oxidation-solidification stabilization restoration agent provided by the invention is simple in components, low in price, easy to obtain and convenient to use.
(2) The oxidation-solidification stabilization repairing agent has a good solidification effect, and soil subjected to solidification stabilization treatment meets IV limit of underground water environment quality standard (GB/T14848-93) and maximum allowable discharge concentration limit of heavy metal of sewage comprehensive discharge standard (GB 5086.1-1996) after being identified by standards such as solid waste leaching toxicity leaching method GB 5086.1-5086.2-1997 and solid waste leaching toxicity determination method GB/T15555.1-15555.12-1995.
Drawings
FIG. 1 is a schematic view of the process flow of the soil oxidation-solidification stabilization of the present invention.
FIG. 2 is a flow chart of the laboratory soil oxidation-solidification stabilization effect test in example 1.
Detailed Description
The technical solutions of the present invention are illustrated below by specific examples, but the scope of the present invention is not limited to the examples.
Example 1
The method comprises the steps of taking polluted soil of a certain PVC production enterprise, and measuring the content of each heavy metal and the content of total Natural Organic Matters (NOM) in the soil, wherein the measurement results of the heavy metals are shown in table 1. It can be found that the content of mercury in the soil exceeds the limit value of 1.5mg/Kg for the mercury content in the tertiary soil in the soil environmental quality Standard (GB15618-1995), and the content of organic matters in the soil is 6 g/Kg.
TABLE 1 heavy metal content in soil and third soil standard limit value mg/kg
The oxidation-solidification stabilization repair agent used in this example was selected from micron-sized zero-valent iron, sodium disilicate, and calcium oxide.
Firstly, crushing the retrieved heavy metal contaminated soil, putting the crushed soil into a plastic cylinder, adding a 10mmol/L sodium disilicate solution and a proper amount of micron zero-valent iron, and fully stirring the mixture while adding the solution, so that the soil is changed into a slurry state. Stirring is continued continuously, proper aeration can be carried out, calcium oxide is added gradually after half an hour, stirring is carried out for 10min, and the experimental device and the brief flow are shown in figure 2. Then placing the slurry in a constant-temperature curing box with the temperature of 60 ℃ and the relative humidity of less than 25% for digestion and molding until the slurry is completely dried and generates certain strength. Digesting and forming for 36h, then naturally cooling, and crushing. Before adding calcium oxide, removing a small amount of slurry, naturally drying, and measuring the content of organic matters in the slurry.
It can be found that after the oxidation process in the previous stage, the content of natural organic matters in the soil is reduced from the original 6g/Kg to 4g/Kg, which indicates that the organic matters in the soil are mineralized and changed into carbon dioxide, and the reduction of the organic matters can reduce the interference on the subsequent soil solidification and stabilization. After the soil subjected to solidification and stabilization treatment is identified by standards such as a solid waste leaching toxicity leaching method GB 5086.1-5086.2-1997 and a solid waste leaching toxicity determination method GB/T15555.1-15555.12-1995, the mercury content of a leaching solution is lower than 0.001mg/L, and the maximum allowable discharge concentration limit (0.05mg/L) of heavy metal mercury in the IV limit (0.001mg/L) of a ground water environment quality standard (GB/T14848-93) and a sewage comprehensive discharge standard (GB 5086.1-1996) is met.
Example 2
the oxidation-solidification stabilization remediation agent adopted in the embodiment is nano-scale zero-valent iron, sodium disilicate and calcium oxide, so as to remediate arsenic-contaminated soil.
Firstly, crushing the retrieved heavy metal contaminated soil, putting the crushed soil into a plastic cylinder (firstly, taking a part of the soil to test the total organic carbon content (TOC)), adding a solution of 20mmol/L sodium disilicate and a proper amount of nano zero-valent iron, and fully stirring the mixture while adding the solution, so that the soil is changed into a slurry state. Stirring is continued continuously, proper aeration can be carried out, calcium oxide is added gradually after half an hour, stirring is carried out for 10min, and the experimental device and the brief flow are shown in figure 2. Then placing the slurry in a constant-temperature curing box with the temperature of 60 ℃ and the relative humidity of less than 25% for digestion and molding until the slurry is completely dried and generates certain strength. Digesting and forming for 36h, then naturally cooling, and crushing. And (3) after the oxidation process is finished and before calcium oxide is added, taking a small amount of slurry, naturally airing, and measuring the TOC value of the slurry.
The result shows that the TOC value of the soil is reduced from the original 500mg/Kg soil to 200mg/Kg soil after the oxidation stage, which shows that the organic matter structure is damaged and mineralized into carbon dioxide. After the soil subjected to solidification and stabilization treatment is identified by standards such as a solid waste leaching toxicity leaching method GB 5086.1-5086.2-1997 and a solid waste leaching toxicity determination method GB/T15555.1-15555.12-1995, the arsenic content of a leaching solution is 0.04mg/L and is lower than 0.05mg/L, and the maximum allowable discharge concentration limit (0.5mg/L) of heavy metal arsenic meets the IV limit (0.05mg/L) of a groundwater environmental quality standard (GB/T14848-93) and a sewage comprehensive discharge standard (GB 5086.1-1996).
Table 2 shows the leaching amounts of As before and after the solidification and stabilization of As-contaminated soil
Example 3
The oxidation-solidification stabilization remediation agent adopted in the embodiment is micron-sized zero-valent iron, sodium disilicate and calcium oxide, so as to remediate the chromium-contaminated soil.
Firstly, crushing the retrieved heavy metal contaminated soil, putting the crushed soil into a plastic cylinder, adding 15mmol/L sodium disilicate solution and a proper amount of micron zero-valent iron, and fully stirring the mixture while adding the solution to obtain slurry-like soil. Stirring is continued continuously and appropriate aeration can be carried out, after half an hour, calcium oxide is added gradually and stirred for 15min, and the experimental device and the brief flow are shown in figure 2. Then placing the slurry in a constant-temperature curing box with the temperature of 60 ℃ and the relative humidity of less than 25% for digestion and molding until the slurry is completely dried and generates certain strength. Digesting and forming for 36h, then naturally cooling, and crushing.
After the soil subjected to solidification and stabilization treatment is identified by standards such as a solid waste leaching toxicity leaching method GB 5086.1-5086.2-1997 and a solid waste leaching toxicity determination method GB/T15555.1-15555.12-1995, the chromium content of a leaching solution is 0.08mg/L and is lower than 0.1mg/L, and the maximum allowable discharge concentration limit (1.5mg/L) of heavy metal chromium meets the IV limit (0.1mg/L) of a groundwater environmental quality standard (GB/T14848-93) and a sewage comprehensive discharge standard (GB 5086.1-1996).
Table 3 shows the leaching amounts of As before and after the stabilization of the chromium-contaminated soil by solidification
Example 4
the oxidation-solidification stabilization remediation agent adopted in the embodiment is micron-sized zero-valent iron, sodium disilicate and calcium oxide, so as to remediate the lead-contaminated soil.
Firstly, crushing the retrieved heavy metal contaminated soil, putting the crushed soil into a plastic cylinder, adding a 20mmol/L sodium disilicate solution and a proper amount of micron zero-valent iron, and fully stirring the mixture while adding the solution, so that the soil is changed into a slurry state. Stirring is continued continuously and appropriate aeration can be carried out, after half an hour, calcium oxide is added gradually, stirring is carried out for 20min, and the experimental device and the brief flow are shown in figure 2. Then placing the slurry in a constant-temperature curing box with the temperature of 60 ℃ and the relative humidity of less than 25% for digestion and molding until the slurry is completely dried and generates certain strength. Digesting and forming for 36h, then naturally cooling, and crushing.
After the soil subjected to solidification and stabilization treatment is identified by standards such as a solid waste leaching toxicity leaching method GB 5086.1-5086.2-1997 and a solid waste leaching toxicity determination method GB/T15555.1-15555.12-1995, the lead content of a leaching solution is 0.08mg/L and is lower than 0.1mg/L, and the maximum allowable discharge concentration limit (1.0mg/L) of heavy metal lead in the IV class limit (0.1mg/L) of a ground water environment quality standard (GB/T14848-93) and a sewage comprehensive discharge standard (GB 5086.1-.
Table 4 shows the leaching amounts of arsenic before and after solidification and stabilization of lead-contaminated soil
Those skilled in the art can implement the present invention in various modifications without departing from the spirit and scope of the present invention, and the above description is only a preferred and feasible embodiment of the present invention, and therefore does not limit the scope of the present invention. Further, it should be understood that various changes or modifications of the present invention may be made by those skilled in the art after reading the teaching of the present invention, and such equivalents may fall within the scope of the present invention as defined in the appended claims.
Claims (4)
1. A method for restoring soil by utilizing a soil oxidation-solidification stabilization restoring agent is characterized by comprising the following steps: firstly, preparing soluble silicate into silicate solution, then adding the silicate solution and zero-valent iron powder into soil to be repaired, and carrying out aeration stirring for more than 0.5 h; then adding a calcium source gradually, and continuing stirring; digesting and forming the slurry after stirring, naturally cooling and crushing to obtain the slurry;
The soil oxidation-solidification stabilization repairing agent comprises the following components: zero-valent iron powder, soluble silicate and a calcium source; the three components are packaged independently.
2. The method of claim 1, wherein: the addition amount of the zero-valent iron powder in each kilogram of soil to be repaired is 0.5-10 g.
3. The method of claim 1, wherein: the addition amount of silicate in each kilogram of soil to be repaired is 0.1-5 g calculated by silicon atom.
4. the method of claim 1, wherein: the soil to be repaired is heavy metal contaminated soil or organic matter-heavy metal combined contaminated soil.
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| CN108031433A (en) * | 2017-12-14 | 2018-05-15 | 湖南科技大学 | A kind of preparation method of mesoporous calcium silicates load nano zero-valence iron composite material |
| CN108326031A (en) * | 2018-01-16 | 2018-07-27 | 航天凯天环保科技股份有限公司 | A kind of method of sulphide staining soil stabilization processing |
| CN109231782A (en) * | 2018-10-17 | 2019-01-18 | 桂林理工大学 | The minimizing stabilization treatment method of Cd in a kind of municipal sludge |
| CN109226243A (en) * | 2018-10-29 | 2019-01-18 | 中国矿业大学(北京) | A kind of the reparation medicament and method of organic-heavy-metal composite pollution soil |
| CN109652080B (en) * | 2019-01-09 | 2020-05-05 | 中国农业大学 | Soil remediation agent and preparation method thereof |
| CN110205134A (en) * | 2019-07-12 | 2019-09-06 | 河南省明创环境科技有限公司 | Medicament using Filling Principle cadmium pollution soil repair and the method using Filling Principle cadmium pollution soil repair |
| CN112250156B (en) * | 2020-10-16 | 2021-10-15 | 中国环境科学研究院 | Silicification modified zero-valent iron and preparation method and application thereof |
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| CN106336869A (en) * | 2016-07-29 | 2017-01-18 | 武汉都市环保工程技术股份有限公司 | Passivating agent used for arsenic polluted soil restoration, arsenic polluted soil restoration method, and application of passivating agent |
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